Interpretable Active Learning for Discovering G‐Quadruplex Deep‐Eutectic Circularly Polarized Luminescence Materials With High Dissymmetry Factor and Quantum Yield

ABSTRACT Circularly polarized luminescence (CPL) materials, which exhibit their unique chiroptical properties, display great potential for applications in optoelectronics and bioimaging. However, it remains a significant challenge to synthesize CPL materials with high dissymmetry factors (g lum ) and photoluminescence quantum yields (PLQY) simultaneously. Herein, we report a deep‐eutectic‐solvent (DES)‐assisted self‐assembly protocol integrated with an active‐learning (AL) framework that enables the targeted fabrication of G‐quadruplex (G4) supramolecular gels with high g lum and PLQY. AL pinpointed the optimal synthesis parameters in just four iterations, dramatically accelerating material development. The top‐performing gel achieved a g lum of 0.29, setting a new benchmark for nucleoside/nucleotide‐based CPL materials. The maximum PLQY reached 10.64%, which represents a substantial level of performance. Furthermore, by integrating SHapley Additive exPlanations (SHAP), we elucidated the relationship between reaction parameters and target properties. Building on this result, we also demonstrated multicolor fluorescence resonance energy transfer (FRET) by incorporating dyes, successfully developing a series of multicolor CPL‐active materials. This work not only provides new insights into the design of bio‐based chiral CPL materials but also highlights the promising role of artificial intelligence in advancing material development.